Multiwalled carbon nanotubes (MWCNTs) were grafted with poly(AMPS-co-AM) by free-radical polymerization of acrylamide (AM) and 2-acrylamido-2-methylpropane sulfonic acid (AMPS) monomers initiated by benzoyl peroxide (BPO). MWCNT-poly(AMPS-co-AM) was characterized by Fourier transform-infrared spectroscopy (FT-IR), thermal gravimetric analysis (TGA), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and energy dispersive spectroscopy (EDS). Observation showed that grafting of poly(AMPS-co-AM) to MWCNTs improves solubility of MWCNTs in water, ethanol, and dichloromethane. MWCNT-poly(AMPS-co-AM) also showed good catalytic performance for the preparation of bis(indolyl)methanes and 1,8-dioxo-octahydroxanthenes through the condensation of an aldehyde with indole and 5,5-dimethyl-1,3-cycloheanedione (dimedone), respectively. MWCNT-poly(AMPS-co-AM) catalyst can be reusable for at least up to eight times without significant loss of activity.